Chiral organic-inorganic hybrid metal halides are a promising class of nonlinear-optical materials with unique optical properties and flexible crystal structures. However, the structures and properties of chiral hybrid tellurium halides, especially second harmonic generation (SHG), have not been reported. Here, by introducing chiral organic molecule (/)-methylbenzylammonium (/-MBA), we synthesized a pair of novel zero-dimensional (0D) chiral tellurium-based hybrid halides with noncentrosymmetric space group 2, (/-MBA)TeCl (). Single-crystal X-ray diffraction analysis and solid-state circular dichroism (CD) spectra confirm that shows obvious enantiomer enrichment. Moreover, the resulting chiral products present an efficient SHG response. Interestingly, through manipulation of halogen atoms, two pairs of achiral tellurium halides, (/-MBA)TeBr () and (/-MBA)TeI (), were obtained, both of which crystallize in the centrosymmetric space group 3̅. It is noteworthy that has a narrow band gap of 1.55 eV, which is smaller than that of most 0D metal halides and comparable to that of three-dimensional lead halide, showing its potential as a highly efficient light absorber.
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